Combined DFT and experiment: Stabilizing the electrochemical interfaces via boron Lewis acids

• 作者: Zhe-Fan Wang Zonglin Yi Aziz Ahmad Lijing Xie Jing-Peng Chen Qingqiang Kong Fangyuan Su Da-Wei Wang Cheng-Meng Chen
• 来源期刊: 能源化学
• 年，卷（期）: 2021,（8）
• 页码范围: 100-107
• 页数: 8页
• 语种: 英文

摘要

The incorporation of boron into carbon material can significantly enhance its capacity performances.However,the origin of the promotion effect of boron doping on electrochemical performances is still unclear,in part due to the inadequate exposure of boron configurations resulting from the complexity of traditional carbon materials.To overcome this issue,herein,a series of boron-doped graphene with highly-exposed boron configurations are prepared by tuning annealing temperature.Then the correlation between boron configurations and the electrochemical performances is investigated.The combination of density-functional theory (DFT) computation and NH3-TPD/Py-FTIR indicates that the BCO2 configuration formed on the surface of graphene is easier to accept lone-pair electrons than BC2O and BC3 configurations due to the stronger Lewis acidity.Such an electronic structure can effectively reduce the number of unstable electron donors and stabilize the electrochemical interface,which is proved by NMR,and critical for improving the electrochemical performances.Further experiments confirm that the optimized BG800 with the largest amount of BCO2 configuration presents ultralow leak current,improved cyclic stability,and better rate performance in SBPBF4/PC.This work would provide an insight into the design of high-performance boron-doped carbon materials towards energy storage.